Data-Driven First-Principles Methods for the Study and Design of Alkali Superionic Conductors
Abstract
We present a detailed exposition of how first-principles methods can be used to guide alkali superionic conductor (ASIC) study and design. Using the argyrodite Li6PS5Cl as a case study, we demonstrate how modern information technology (IT) infrastructure and software tools can facilitate the assessment of alkali superionic conductors in terms of various critical properties of interest such as phase and electrochemical stability and ionic conductivity. The emphasis is on well-documented, reproducible analysis code that can be readily generalized to other material systems and design problems. For our chosen Li6PS5Cl case study material, we show that Li excess is crucial to enhancing its conductivity by increasing the occupancy of interstitial sites that promote long-range Li+ diffusion between cage-like frameworks. The predicted room-temperature conductivities and activation barriers are in reasonably good agreement with experimental values.
- Authors:
-
- Univ. of California, San Diego, CA (United States)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1479673
- Grant/Contract Number:
- SC0012118
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemistry of Materials
- Additional Journal Information:
- Journal Volume: 29; Journal Issue: 1; Journal ID: ISSN 0897-4756
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 42 ENGINEERING; 97 MATHEMATICS AND COMPUTING
Citation Formats
Deng, Zhi, Zhu, Zhuoying, Chu, Iek-Heng, and Ong, Shyue Ping. Data-Driven First-Principles Methods for the Study and Design of Alkali Superionic Conductors. United States: N. p., 2016.
Web. doi:10.1021/acs.chemmater.6b02648.
Deng, Zhi, Zhu, Zhuoying, Chu, Iek-Heng, & Ong, Shyue Ping. Data-Driven First-Principles Methods for the Study and Design of Alkali Superionic Conductors. United States. https://doi.org/10.1021/acs.chemmater.6b02648
Deng, Zhi, Zhu, Zhuoying, Chu, Iek-Heng, and Ong, Shyue Ping. Sat .
"Data-Driven First-Principles Methods for the Study and Design of Alkali Superionic Conductors". United States. https://doi.org/10.1021/acs.chemmater.6b02648. https://www.osti.gov/servlets/purl/1479673.
@article{osti_1479673,
title = {Data-Driven First-Principles Methods for the Study and Design of Alkali Superionic Conductors},
author = {Deng, Zhi and Zhu, Zhuoying and Chu, Iek-Heng and Ong, Shyue Ping},
abstractNote = {We present a detailed exposition of how first-principles methods can be used to guide alkali superionic conductor (ASIC) study and design. Using the argyrodite Li6PS5Cl as a case study, we demonstrate how modern information technology (IT) infrastructure and software tools can facilitate the assessment of alkali superionic conductors in terms of various critical properties of interest such as phase and electrochemical stability and ionic conductivity. The emphasis is on well-documented, reproducible analysis code that can be readily generalized to other material systems and design problems. For our chosen Li6PS5Cl case study material, we show that Li excess is crucial to enhancing its conductivity by increasing the occupancy of interstitial sites that promote long-range Li+ diffusion between cage-like frameworks. The predicted room-temperature conductivities and activation barriers are in reasonably good agreement with experimental values.},
doi = {10.1021/acs.chemmater.6b02648},
journal = {Chemistry of Materials},
number = 1,
volume = 29,
place = {United States},
year = {Sat Sep 03 00:00:00 EDT 2016},
month = {Sat Sep 03 00:00:00 EDT 2016}
}
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